Monte-Carlo Simulations of Spin-Crossover Phenomena Based on a Vibronic Ising-like Model with Realistic Parameters

Materials with spin-crossover (SCO) properties hold great potentials in information storage and therefore have received a lot of concerns in the recent decades. The hysteresis phenomena accompanying SCO is attributed to the intermolecular cooperativity whose underlying mechanism may have a vibronic origin. In this work, a new vibronic Ising-like model in which the elastic coupling between SCO centers is included by considering harmonic stretching and bending (SAB) interactions is proposed and solved by Monte Carlo simulations. The key parameters in the new model, $k_1$ and $k_2$, corresponding to the elastic constant of the stretching and bending mode, respectively, can be directly related to the macroscopic bulk and shear modulus of the material in study, which can be readily estimated either based on experimental measurements or first-principles calculations. The convergence issue in the MC simulations of the thermal hysteresis has been carefully checked, and it was found that the stable hysteresis loop can be more readily obtained when using the SAB model compared to that using the Wajnflasz-Pick model. Using realistic parameters estimated based on first-principles calculations of a specific polymeric coordination SCO compound, [Fe(pz)Pt(CN)$_4$]$\cdot$2H$_2$O, temperature-induced hysteresis and pressure effects on SCO phenomena are simulated successfully.Comment: 8 pages, 8 figure

Optical isolation with nonlinear topological photonics

It is shown that the concept of topological phase transitions can be used to design nonlinear photonic structures exhibiting power thresholds and discontinuities in their transmittance. This provides a novel route to devising nonlinear optical isolators. We study three representative designs: (i) a waveguide array implementing a nonlinear 1D Su-Schrieffer-Heeger (SSH) model, (ii) a waveguide array implementing a nonlinear 2D Haldane model, and (iii) a 2D lattice of coupled-ring waveguides. In the first two cases, we find a correspondence between the topological transition of the underlying linear lattice and the power threshold of the transmittance, and show that the transmission behavior is attributable to the emergence of a self-induced topological soliton. In the third case, we show that the topological transition produces a discontinuity in the transmittance curve, which can be exploited to achieve sharp jumps in the power-dependent isolation ratio.Comment: 11 pages, 7 figure

Ultrafast and octave-spanning optical nonlinearities from strongly phase-mismatched cascaded interactions

Cascaded nonlinearities have attracted much interest, but ultrafast applications have been seriously hampered by the simultaneous requirements of being near phase-matching and having ultrafast femtosecond response times. Here we show that in strongly phase-mismatched nonlinear frequency conversion crystals the pump pulse can experience a large and extremely broadband self-defocusing cascaded Kerr-like nonlinearity. The large cascaded nonlinearity is ensured through interaction with the largest quadratic tensor element in the crystal, and the strong phase-mismatch ensures an ultrafast nonlinear response with an octave-spanning bandwidth. We verify this experimentally by showing few-cycle soliton compression with noncritical cascaded second-harmonic generation: Energetic 47 fs infrared pulses are compressed in a just 1-mm long bulk lithium niobate crystal to 17 fs (under 4 optical cycles) with 80% efficiency, and upon further propagation an octave-spanning supercontinuum is observed. Such ultrafast cascading is expected to occur for a broad range of pump wavelengths spanning the near- and mid-IR using standard nonlinear crystals.Comment: resubmitted, revised version, accepted for Phys. Rev. Let